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Highly sensitive characterization of surface plasmon resonance (SPR) modes lays the solid foundation for wide SPR-related applications. Herein, we discover that these SPR modes based on all-metal nanostructures without any probed molecule can be characterized with ultrahigh sensitivities at both excitation and emission wavelengths by utilizing plasmon-enhanced sum frequency generation (PESFG) spectroscopy. The theory of PESFG for sensitively characterizing SPR modes is first validated experimentally. Moreover, we have elaborately demonstrated that PESFG strongly depends on both the resonant wavelengths of SPR modes and spatial mode distributions when azimuthal angles of excitations are varied. Our study not only enhances the understanding of the mechanism that governs PESFG, but also offers a potentially new method for exploring new-style SPR modes (e.g. plasmon-induced magnetic resonance and bound states in the continuum) by PESFG.